Abstract
The fundamental unit for comprehending the physicochemical properties of water, the Zundel cation configuration H5O2+, has yet to be exhaustively evaluated in terms of its interaction with terahertz (THz) electromagnetic waves, characterized by sub-picosecond oscillation periods or pulse widths. In this study, we embark on an investigation of the broad resonance and high-field nonresonant effects of intense THz radiation (ITR) on Zundel cations, utilizing a multifaceted methodological approach that includes density functional theory (DFT) calculations, finite difference time domain (FDTD) algorithm of the Schrödinger equation, and ab initio molecular dynamics (AIMD) simulations. Our analysis reveals that the proton potential energy surface (PES) varies in response to the external electric (E) field, suggesting that the interaction frequency of the central proton with the electromagnetic wave encompasses the THz band. This resonance effect is associated with proton behavior that may oscillate or demonstrate periodic tunneling. Moreover, our work uncovers the high-field nonresonant effects of ITR on Zundel cations, manifesting in proton transfer and vibrational excitation of the system. Our findings contribute to the understanding of the interaction between Zundel species and electromagnetic waves by presenting a microscopic view of proton transfer as informed by wavefunction evolution.